Structured electrodes with tailored nanoscale morphology and chemistry are highly desirable for a range of applications. In particular, emerging energy storage applications such as thick Lithium-ion battery (LIB) electrodes and photoanodes for watersplitting require new electrode structures that simultaneously optimise electron, ion, and thermal transport. In this PhD thesis, advanced structured electrodes are fabricated by creating 3D carbon-inorganic hybrid architectures. In this process, patterned vertically aligned carbon nanotubes (CNT) were used as the structural scaffolds to shape the electrodes while inheriting the excellent thermal and electrical properties of CNTs.

First, UV and colloidal lithographic patterning processes were developed to create micro- and nanopores respectively within the CNT structures. Those structures provide high surface area and conductive backbone for the synthesis of hybrid CNT-inorganic structures. Specifically, the parameter space to create honeycomb shaped CNT structures with pores ranging from 300~nm to 30~$\mu$m has been established.

Next, the micro-pore CNT structures have been chemically modified with iron oxide using microwave-assisted, hydrothermal synthesis for fabricating high areal loading LIB anodes. The areal loading was increased by 120% compared to a standard battery film while at the same time retaining a high capacity (900 mAhg$\mathrm{<mrow\; data-mjx-texclass="ORD">-1</mrow>}$ at 0.2 C). Then thick electrodes with optimised diffusion pathways were created by coating the nanopatterned CNTs with silicon using physical vapour deposition. These electrode structures are up to 50% thicker than previously reported structures and still retain a stable capacity (650 mAhg$\mathrm{<mrow\; data-mjx-texclass="ORD">-1</mrow>}$) and a good high-rate performance. Finally, the honeycomb shaped CNT structures have been coated with bismuth vanadate using a hotcasting process and the electrode architecture has been optimized for good conductivity by the addition of a Pd/Au layer between the CNTs and the BiVO$\mathrm{<mrow\; data-mjx-texclass="ORD">4</mrow>}$. The photoelectrode performance was measured and shows a clear increase in current density when exposed to light.

Each of these novel electrodes illustrate how patterning vertically aligned carbon nanotube structures combined with inorganic surface modification enables the creation of advanced electrodes with new formfactors and improved performance in comparison to literature and to classic drop-casted battery films of the same materials.